Related papers: Nonadiabatic Ehrenfest molecular dynamics within t…
Nonadiabatic effects that arise from the concerted motion of electrons and atoms at comparable energy and time scales are omnipresent in thermal and light-driven chemistry at metal surfaces. Excited (hot) electrons can measurably affect…
We have employed non-adiabatic molecular dynamics based on time-dependent density-functional theory to characterize the scattering behaviour of a proton with the Li$_4$ cluster. This technique assumes a classical approximation for the…
We study the gas-surface dynamics of O2 at Ag(111) with the particular objective to unravel whether electronic non-adiabatic effects are contributing to the experimentally established inertness of the surface with respect to oxygen uptake.…
The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one and three dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. We consider three…
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified,…
We present an implementation of optimal control theory for the first-principles non-adiabatic Ehrenfest Molecular Dynamics model, which describes a condensed matter system by considering classical point-particle nuclei, and quantum…
The Projected Augmented Waves (PAW) method is based on a linear transformation between the pseudo wavefunctions and the all electron wavefunctions. To obtain high accuracy with this method, it is important that the local part of the linear…
We focus in this work on the numerical discretization of the one dimensional aggregation equation $\pa_t\rho + \pa_x (v\rho)=0$, $v=a(W'*\rho)$, in the attractive case. Finite time blow up of smooth initial data occurs for potential $W$…
Quantum molecular dynamics requires an accurate representation of the molecular potential energy surface from a minimal number of electronic structure calculations, particularly for nonadiabatic dynamics where excited states are required.…
The propagation of electromagnetic waves in general media is modeled by the time-dependent Maxwell's partial differential equations (PDEs), coupled with constitutive laws that describe the response of the media. In this work, we focus on…
It was recently shown [Phys. Rev. Lett. 105, 123002 (2010)] that the complete wavefunction for a system of electrons and nuclei evolving in a time-dependent external potential can be exactly factorized into an electronic wavefunction and a…
The Ehrenfest urn process, also known as the dogs and fleas model, is realistically simulated by molecular dynamics of the Lennard-Jones fluid. The key variable is Delta z, i.e. the absolute value of the difference between the number of…
The exact factorization (EF) approach to coupled electron-ion dynamics recasts the time-dependent molecular Schr\"odinger equation as two coupled equations, one for the nuclear wavefunction and one for the conditional electronic…
With recent developments in simulating nonadiabatic systems to high accuracy, it has become possible to determine how much energy is attributed to nuclear quantum effects beyond zero-point energy. In this work we calculate the…
We develop a general method allowing one to construct the consistent theory of light pulse propagation through an atomic medium in arbitrary nonlinear regime with respect to the field strength, taking into account the light polarization,…
We discuss nuclear dynamics at molecule-metal interfaces including non-equilibrium molecular junctions. Starting from the many-body states (pseudoparticle) formulation of the molecule-metal system in the molecular vibronic basis, we…
We propose to measure nonadiabaticity of molecular quantum dynamics rigorously with the quantum fidelity between the Born-Oppenheimer and fully nonadiabatic dynamics. It is shown that this measure of nonadiabaticity applies in situations…
Ehrenfest, Born-Oppenheimer, Langevin and Smoluchowski dynamics are shown to be accurate approximations of time-independent Schr\"odinger observables for a molecular system avoiding caustics, in the limit of large ratio of nuclei and…
We first discuss the geometrical construction and the main mathematical features of the maximum-entropy-production/steepest-entropy-ascent nonlinear evolution equation proposed long ago by this author in the framework of a fully quantum…
We discuss time dependent quantum systems on bounded domains. Our work may be viewed as a framework for several models, including linear iterations involved in time dependent density functional theory (TDDFT), the Hartree-Fock model, or…